A FeCuNbSiB/FeNi/PZT laminated composite is developed and comparatively studied with a FeNi/PZT laminated composite. The influence of high-permeability FeCuNbSiB alloy on applied DC magnetic field, piezomagnetic coefficient and optimal bias magnetic field of FeNi is investigated. The experimental results show that compared with in the two-phase FeNi/PZT, in the three-phase FeCuNbSiB/FeNi/PZT laminated composite, (i) the optimal bias magnetic field decreases from 200Oe to 55Oe, and the maximum magnetoelectric(ME) voltage coefficient increases from 1.59V/Oe to 2.77V/Oe; (ii) under small bias magnetic field, the ME voltage coefficient increases by a factor of 1.7—7.8; (iii) the sensitivity of the ME voltage coefficient for the laminated composite to a DC magnetic field increases from 19.1mV/Oe to 158.6mV/Oe. The variations in ME effect of three-phase composie result from the enhancement of magnetizetion at end faces, which is generated by introducing the high permeability material phase.